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Many-body screening effects in liquid water

The screening arising from many-body excitations is a crucial quantity for describing absorption and inelastic X-ray scattering (IXS) of materials. Similarly, the electron screening plays a critical role in state-of-the-art approaches for determining the fundamental band gap. However, ab initio stud...

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Autores principales: Reshetnyak, Igor, Lorin, Arnaud, Pasquarello, Alfredo
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2023
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10175292/
https://www.ncbi.nlm.nih.gov/pubmed/37169764
http://dx.doi.org/10.1038/s41467-023-38420-w
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author Reshetnyak, Igor
Lorin, Arnaud
Pasquarello, Alfredo
author_facet Reshetnyak, Igor
Lorin, Arnaud
Pasquarello, Alfredo
author_sort Reshetnyak, Igor
collection PubMed
description The screening arising from many-body excitations is a crucial quantity for describing absorption and inelastic X-ray scattering (IXS) of materials. Similarly, the electron screening plays a critical role in state-of-the-art approaches for determining the fundamental band gap. However, ab initio studies of the screening in liquid water have remained limited. Here, we use a combined analysis based on the Bethe-Salpeter equation and time-dependent density functional theory. We first show that absorption spectra at near-edge energies are insufficient to assess the accuracy by which the screening is described. Next, when the energy range under scrutiny is extended, we instead find that the IXS spectra are highly sensitive and allow for the selection of the optimal theoretical scheme. This leads to good agreement with experiment over a large range of transferred energies and momenta, and enables establishing the elusive fundamental band gap of liquid water at 9.3 eV.
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spelling pubmed-101752922023-05-13 Many-body screening effects in liquid water Reshetnyak, Igor Lorin, Arnaud Pasquarello, Alfredo Nat Commun Article The screening arising from many-body excitations is a crucial quantity for describing absorption and inelastic X-ray scattering (IXS) of materials. Similarly, the electron screening plays a critical role in state-of-the-art approaches for determining the fundamental band gap. However, ab initio studies of the screening in liquid water have remained limited. Here, we use a combined analysis based on the Bethe-Salpeter equation and time-dependent density functional theory. We first show that absorption spectra at near-edge energies are insufficient to assess the accuracy by which the screening is described. Next, when the energy range under scrutiny is extended, we instead find that the IXS spectra are highly sensitive and allow for the selection of the optimal theoretical scheme. This leads to good agreement with experiment over a large range of transferred energies and momenta, and enables establishing the elusive fundamental band gap of liquid water at 9.3 eV. Nature Publishing Group UK 2023-05-11 /pmc/articles/PMC10175292/ /pubmed/37169764 http://dx.doi.org/10.1038/s41467-023-38420-w Text en © The Author(s) 2023 https://creativecommons.org/licenses/by/4.0/Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/ (https://creativecommons.org/licenses/by/4.0/) .
spellingShingle Article
Reshetnyak, Igor
Lorin, Arnaud
Pasquarello, Alfredo
Many-body screening effects in liquid water
title Many-body screening effects in liquid water
title_full Many-body screening effects in liquid water
title_fullStr Many-body screening effects in liquid water
title_full_unstemmed Many-body screening effects in liquid water
title_short Many-body screening effects in liquid water
title_sort many-body screening effects in liquid water
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10175292/
https://www.ncbi.nlm.nih.gov/pubmed/37169764
http://dx.doi.org/10.1038/s41467-023-38420-w
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